Impact of Secondary Sphere Hydrogen Bonds on O2 Reactivity within a Nonheme Iron Complex DOI

Andrew R. LaDuca,

Jessica R. Wilson, Writhabrata Sarkar

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 2, 2025

A nonheme iron complex bearing the tris(6-phenylamino-pyridyl)methylamine (TPANHPh) ligand with appended hydrogen bond (H-bond) groups displays facile O2 reactivity to form a monomeric Fe(III)OH complex, which can release •OH via rebound carbon radical. An analogous compound without H-bonds, based on tris(6-methylpyridyl)methylamine (TPAMe), exhibits minimal reactivity, forming Fe(III)2(μ-O)(μ–OH) dimer, also reacts carbon-based radicals. The H-bonding system enables binding and activation at weakly reducing complexes, highlighting cooperative role of secondary sphere units facilitate reactions atypical redox environments.

Language: Английский

Impact of Secondary Sphere Hydrogen Bonds on O2 Reactivity within a Nonheme Iron Complex DOI

Andrew R. LaDuca,

Jessica R. Wilson, Writhabrata Sarkar

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 2, 2025

A nonheme iron complex bearing the tris(6-phenylamino-pyridyl)methylamine (TPANHPh) ligand with appended hydrogen bond (H-bond) groups displays facile O2 reactivity to form a monomeric Fe(III)OH complex, which can release •OH via rebound carbon radical. An analogous compound without H-bonds, based on tris(6-methylpyridyl)methylamine (TPAMe), exhibits minimal reactivity, forming Fe(III)2(μ-O)(μ–OH) dimer, also reacts carbon-based radicals. The H-bonding system enables binding and activation at weakly reducing complexes, highlighting cooperative role of secondary sphere units facilitate reactions atypical redox environments.

Language: Английский

Citations

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